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Cu surface plasmon resonance promoted charge transfer in S-scheme system enhanced visible light photocatalytic hydrogen evolution 铜表面等离子体共振促进了 S 型体系中的电荷转移,增强了可见光光催化氢气进化。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1016/j.jcis.2024.10.087
Reasonably constructing nanocomposite photocatalysts with fast charge transfer and broad solar response capabilities is significant for efficiently converting solar energy into chemical energy. Cu modifies P25/CeO2 heterojunctions prepared by photodeposition (P25 is commercial TiO2). The local surface plasmon resonance (LSPR) effect caused by Cu nanoparticles broadens the spectral response range and generates significant photothermal effects. After 90 s of irradiation, the temperature of 9.5 %Cu-P25/CeO2 increases to 148.1 °C. The photocatalytic hydrogen evolution rate (HER) of 9.5 %Cu-P25/CeO2 under visible light (λ = 400 nm) reaches 1538.2 μmol h−1 g−1, which is 158.6 times, 17.7 times, and 2.5 times higher than that of Cerium dioxide (CeO2), P25, and P25/CeO2, respectively. This catalyst has stronger light absorption, easier carrier transfer, and separation. This study guides the construction of efficient hydrogen evolution photocatalysts.
合理构建具有快速电荷转移和广泛太阳能响应能力的纳米复合光催化剂,对于高效地将太阳能转化为化学能具有重要意义。铜对通过光沉积制备的 P25/CeO2 异质结(P25 为商用 TiO2)进行了改性。铜纳米粒子引起的局部表面等离子体共振(LSPR)效应拓宽了光谱响应范围,并产生了显著的光热效应。辐照 90 秒后,9.5%Cu-P25/CeO2 的温度升至 148.1 °C。在可见光(λ = 400 nm)下,9.5 %Cu-P25/CeO2 的光催化氢进化率(HER)达到 1538.2 μmol h-1 g-1,分别是二氧化铈(CeO2)、P25 和 P25/CeO2 的 158.6 倍、17.7 倍和 2.5 倍。这种催化剂具有更强的光吸收能力,更易于载流子的转移和分离。这项研究为构建高效氢进化光催化剂提供了指导。
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引用次数: 0
A review of ordered PtCo3 catalyst with higher oxygen reduction reaction activity in proton exchange membrane fuel cells 质子交换膜燃料电池中具有更高氧还原反应活性的有序钴铂催化剂综述。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1016/j.jcis.2024.10.063
This review is devoted to the potential advantages of ordered alloy catalysts in proton exchange membrane fuel cells (PEMFCs), specifically focusing on the development of the low Pt content, high activity, and durability ordered PtCo3 catalyst. Due to the sluggish oxygen reduction reaction (ORR) kinetics and poor durability, the overall performance of the fuel cell is affected, and its application and promotion are limited. To address this issue, researchers have explored various synthetic strategies, such as element doping, morphology adjusting, structure controlling, ordering and support/metal interaction enhancement. This article extensively discussed the Pt related ORR catalysts and follows an in-depth analysis of ordered PtCo3. The introduction briefly discusses the direction of development of fuel cell catalysts and frontier progress, including theoretical mechanism, practical preparation, and Pt-containing electrode structures, etc. The subsequent chapter focuses on the Pt-Co catalyst, the evolution process of Pt alloy to Pt-Co alloy and the improvement scheme are introduced. The next chapter describes the properties of PtCo3. Although the ordered PtCo3 catalyst has a wide range of applicability due to low cost and high activity catalyst. However, besides the common agglomeration and sintering problems of Pt-Co alloy, its commercial application still faces unique problems of oversized crystal size, phase segregation, ordering transformation and transition metal dissolution. Therefore, in Chapter 4, this overview provides some possible improvement methods for three specific functions: crystal refinement, enhancing the effect of support and active substances, and anti-dissolution.
本综述专门讨论有序合金催化剂在质子交换膜燃料电池(PEMFC)中的潜在优势,尤其侧重于低铂含量、高活性和耐久性有序钴铂催化剂的开发。由于氧还原反应(ORR)动力学迟缓、耐久性差,燃料电池的整体性能受到影响,其应用和推广受到限制。针对这一问题,研究人员探索了多种合成策略,如元素掺杂、形貌调整、结构控制、有序化和支撑/金属相互作用增强等。本文广泛讨论了与铂有关的 ORR 催化剂,并对有序 PtCo3 进行了深入分析。引言简要论述了燃料电池催化剂的发展方向和前沿进展,包括理论机理、实际制备、含铂电极结构等。随后一章重点介绍了铂-钴催化剂,介绍了铂合金向铂-钴合金的演化过程和改进方案。下一章介绍了 PtCo3 的特性。尽管有序 PtCo3 催化剂因其低成本和高活性催化剂而具有广泛的适用性。然而,除了铂钴合金常见的团聚和烧结问题外,其商业应用还面临着晶体尺寸过大、相分离、有序转变和过渡金属溶解等独特问题。因此,本综述将在第 4 章中针对晶体细化、增强支撑和活性物质的效果以及防溶解这三个具体功能提供一些可行的改进方法。
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引用次数: 0
The role of lignin as interfacial compatibilizer in designing lignocellulosic-polyester composite films 木质素作为界面相容剂在设计木质纤维素-聚酯复合薄膜中的作用。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1016/j.jcis.2024.10.083
Advancing nanocomposites requires a deep understanding and careful design of nanoscale interfaces, as interfacial interactions and adhesion significantly influence the physical and mechanical properties of these materials. This study demonstrates the effectiveness of lignin nanoparticles (LNPs) as interfacial compatibilizer between hydrophilic cellulose nanofibrils (CNF) and a hydrophobic polyester, polycaprolactone (PCL). In this context, we conducted a detailed analysis of surface-to-bulk interactions in both wet and dry conditions using advanced techniques such as quartz crystal microbalance with dissipation (QCM-D), atomic force microscopy (AFM), water contact angle (WCA) measurements, broadband dielectric spectroscopy (BDS), and inverse gas chromatography (IGC).
QCM-D was employed to quantify the adsorption behavior of LNPs on CNF and PCL surfaces, demonstrating LNPs’ capability to interact with both hydrophilic and hydrophobic phases, thereby enhancing composite material properties. LNPs showed extensive adsorption on a CNF model film (1186 ± 178 ng.cm−2) and a lower but still significant adsorption on a PCL model film (270 ± 64 ng.cm−2). In contrast, CNF adsorption on a PCL model film was the lowest, with a sensed mass of only 136 ± 35 ng.cm−2. These findings were further supported by comparing the morphology and wettability of the films before and after adsorption, using AFM and WCA analyses. Then, to gain insights into the molecular-level interactions and molecular mobility within the composite in dry state, BDS was employed. The BDS results showed that LNPs improved the dispersion of PCL within the CNF network. To further investigate the impact of LNPs on the composites’ interfacial properties, IGC was employed. This analysis showed that the composite films containing LNPs exhibited lower surface energy compared to those composed of only CNF and PCL. The presence of LNPs likely reduced the availability of surface hydroxyl groups, thus modifying the physicochemical properties of the interface. These changes were particularly evident in the heterogeneity of the surface energy profile, indicating that LNPs significantly altered the interfacial characteristics of the composite materials.
Overall, these findings emphasize the necessity to control the interfaces between components for next-generation nanocomposite materials across diverse applications.
要推进纳米复合材料的发展,就必须深入了解并精心设计纳米级界面,因为界面相互作用和附着力会极大地影响这些材料的物理和机械性能。本研究证明了木质素纳米颗粒(LNPs)作为亲水性纤维素纳米纤维(CNF)和疏水性聚酯聚己内酯(PCL)之间的界面相容剂的有效性。在这种情况下,我们采用先进的技术,如带耗散的石英晶体微天平 (QCM-D)、原子力显微镜 (AFM)、水接触角 (WCA) 测量、宽带介电光谱 (BDS) 和反气相色谱法 (IGC),详细分析了湿和干条件下表面与聚合物之间的相互作用。QCM-D 被用来量化 LNPs 在 CNF 和 PCL 表面上的吸附行为,证明 LNPs 能够与亲水相和疏水相相互作用,从而增强复合材料的性能。LNPs 在 CNF 模型薄膜上的吸附量很大(1186 ± 178 ng.cm-2),而在 PCL 模型薄膜上的吸附量较小,但仍很显著(270 ± 64 ng.cm-2)。相比之下,CNF 在 PCL 模型薄膜上的吸附量最低,感应质量仅为 136 ± 35 ng.cm-2。利用原子力显微镜和 WCA 分析比较了吸附前后薄膜的形态和润湿性,进一步证实了上述发现。然后,为了深入了解干燥状态下复合材料内部的分子水平相互作用和分子流动性,采用了 BDS 方法。BDS 结果表明,LNPs 改善了 PCL 在 CNF 网络中的分散性。为了进一步研究 LNPs 对复合材料界面特性的影响,采用了 IGC 分析法。该分析表明,与仅由 CNF 和 PCL 组成的复合薄膜相比,含有 LNPs 的复合薄膜表现出较低的表面能。LNPs 的存在可能降低了表面羟基的可用性,从而改变了界面的物理化学特性。这些变化在表面能分布的异质性中尤为明显,表明 LNPs 显著改变了复合材料的界面特性。总之,这些发现强调了在各种应用中控制下一代纳米复合材料各组分之间界面的必要性。
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引用次数: 0
Tannic acid etching construction of hollow heterogeneous CoSe2-FeSe2@nitrogen-doped carbon rhombic dodecahedron for high-performance sodium storage 鞣酸蚀刻构建用于高性能钠储存的中空异质 CoSe2-FeSe2@ 掺氮碳菱形十二面体。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1016/j.jcis.2024.10.081
Metal selenides are very promising anode materials for sodium ion batteries (SIBs) due to their rich redox behaviors, low cost, high theoretical capacity, and environmentally benign. However, the poor cycle performance and rate capability greatly hinder their widespread applications. In this paper, we have proposed a tannic acid etching zeolitic imidazolate framework-67 (ZIF-67)-derived selenide strategy to construct hollow heterogeneous CoSe2-FeSe2@N-doped carbon rhombic dodecahedron (CoSe2-FeSe2@NC) as anode for high-performance SIBs. The special microstructural characteristics with hollow rhombic dodecahedron can reduce the Na+/electron migration path and alleviate the volume variations during cycling. The NC can improve conductivity and reduce volume effects during cycling. What’s more, the built-in electric fields (BIEF) at the CoSe2-FeSe2 heterointerfaces can modulate the electronic structure and accelerate the kinetics of ionic diffusion, resulting in the improvement electrochemical properties. When applied as anodes for SIBs, the CoSe2-FeSe2@NC can deliver a remarkable electrochemical performance in terms of sodium storage capacity (648.5 mAh g−1 at 0.2 A/g), initial coulombic efficiency (82.0 %), cycle performance (92.6 % capacity retention after 100 cycles), and rate capability of 450.6 mAh g−1 after 1000 cycles at a high rate of 1 A/g. The kinetic analysis indicates that the discharging-charging process of CoSe2-FeSe2@NC is ascribed to both capacitive behavior and controlled diffusion.
金属硒化物具有丰富的氧化还原行为、成本低、理论容量高且对环境无害,是非常有前途的钠离子电池(SIB)正极材料。然而,较差的循环性能和速率能力极大地阻碍了它们的广泛应用。本文提出了一种单宁酸蚀刻沸石咪唑酸框架-67(ZIF-67)衍生硒化物的策略,以构建中空异质 CoSe2-FeSe2@N 掺杂碳菱形十二面体(CoSe2-FeSe2@NC)作为高性能 SIB 的阳极。中空十二面体的特殊微观结构特征可以减少 Na+/电子迁移路径,缓解循环过程中的体积变化。NC 可以提高导电性,减少循环过程中的体积效应。此外,CoSe2-FeSe2 异质界面上的内置电场(BIEF)可以调节电子结构,加速离子扩散动力学,从而改善电化学性能。将 CoSe2-FeSe2@NC 用作 SIB 的阳极时,其钠存储容量(0.2 A/g 时为 648.5 mAh g-1)、初始库仑效率(82.0%)、循环性能(100 次循环后容量保持率为 92.6%)以及 1 A/g 高倍率下 1000 次循环后 450.6 mAh g-1 的速率能力等方面的电化学性能都非常出色。动力学分析表明,CoSe2-FeSe2@NC 的放电-充电过程可归因于电容行为和受控扩散。
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引用次数: 0
Easy reversible clustering of gold nanoparticles via pH-Induced assembly of PVP-b-PAA copolymer 通过 PVP-b-PAA 共聚物的 pH 值诱导组装,轻松实现金纳米粒子的可逆聚类。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1016/j.jcis.2024.10.068
The growing demand of novel hybrid organic/inorganic systems with exciting properties has contributed to an increasing need for simplifying production strategies. Here, we report a simple method to obtain controlled three-dimensional hybrid architectures, in particular hybrid supracolloids (hSC), formed by gold nanoparticles and a double hydrophilic block copolymer, specifically the poly(acrylic acid)-block-poly(N-vinyl-2-pyrrolidone) (PAA-b-PVP), directly in aqueous medium. The ubiquitous pH-sensitive poly(acrylic acid) (PAA) block initiates the assembly through pH changes, while the poly(N-vinyl-2-pyrrolidone) block assures the close affinity with the AuNPs. We demonstrate that the formation of hybrid supracolloids (hSC) is the result of the synergetic behavior of the two specific polymeric blocks. Additionally, the entire process shows spontaneous and fast switchability. The nanostructured copolymer behaves like a highly swollen hydrogel and displays a disordered internal structure. The driving force for the association of the copolymer chains is induced by the synergetic effects of the decrease in solubility of the poly(acrylic acid) block and the formation of inter and intra chains hydrogen bonds. These were demonstrated by using small angle X-ray scattering (SAXS), quartz crystal microbalance with dissipation monitoring (QCM-D) and scanning transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy (STEM-EDX). In turn, the AuNPs are randomly spread all over the polymeric matrix, as demonstrated by field emission gun – scanning electron microscopy (FEG-SEM). A correlation analysis reveals the hSC density depends mostly on the initial concentration of AuNPs. These results can inspire the fabrication of more complex structures with multicomponent composition.
对具有令人兴奋的特性的新型有机/无机杂化体系的需求日益增长,这促使对简化生产策略的需求与日俱增。在此,我们报告了一种在水介质中直接获得可控三维杂化体系结构,特别是由金纳米粒子和双亲水嵌段共聚物(特别是聚(丙烯酸)-嵌段-聚(N-乙烯基-2-吡咯烷酮)(PAA-b-PVP))形成的杂化超球体(hSC)的简单方法。无处不在的对 pH 值敏感的聚(丙烯酸)(PAA)嵌段通过 pH 值变化启动组装,而聚(N-乙烯基-2-吡咯烷酮)嵌段则确保了与 AuNPs 的紧密亲和性。我们证明,杂化超胶体(hSC)的形成是两种特定聚合物嵌段协同作用的结果。此外,整个过程显示出自发和快速的可切换性。纳米结构共聚物的行为类似于高度膨胀的水凝胶,并显示出无序的内部结构。共聚物链结合的驱动力来自于聚丙烯酸嵌段溶解度的降低以及链间和链内氢键的形成所产生的协同效应。小角 X 射线散射(SAXS)、石英晶体微天平耗散监测(QCM-D)和扫描透射电子显微镜耦合能量色散 X 射线光谱(STEM-EDX)证明了这一点。反过来,场发射枪-扫描电子显微镜(FEG-SEM)也证明了 AuNPs 在聚合物基质中的随机分布。相关分析表明,hSC 密度主要取决于 AuNPs 的初始浓度。这些结果可以启发人们制造具有多组分成分的更复杂结构。
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引用次数: 0
One-step fabrication of a novel fiber-based absorber for flexible, tunable and boosted microwave absorption 一步法制造新型光纤吸收器,实现灵活、可调和增强的微波吸收。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1016/j.jcis.2024.10.072
The increasingly intricate electromagnetic environment necessitates higher anti-electromagnetic interference capabilities for electronic devices, thereby demanding a flexible absorbing material that can adapt to multiple forms, is lightweight, and exhibits excellent electromagnetic wave (EMW) absorption properties. In this study, we have developed a novel flexible absorbing material (FAM) based on glass-coated amorphous magnetic fibers (SFs) and Dallenbach-like absorbing structures through wet forming technology. By combining high-performance absorbing fiber with textile structures, the FAM demonstrates EMW absorption performance along with lightweight flexibility and shape adaptability. This paper explores the influence of process parameters in wet forming technology on FAM formation; as well as examines the construction of broadband absorbers through structural optimization. A single-layer FAM with a thickness of 1.7 mm (SFs length 8 mm, content 3 g/m2) achieves an impressive reflection loss (RL) value of −60.1 dB at 11.6 GHz. Furthermore, optimized multi-layer FAM attains effective absorption bandwidth (EAB: RL ≤ −5 dB) across a wide range from 3 to 14 GHz. This work presents a new approach for developing ’lightweight, thin, wide, and strong’ absorbing materials based on fiber and textile structures which holds significant implications for civilian electromagnetic interference protection as well as military electromagnetic stealth technology.
日益复杂的电磁环境要求电子设备具有更高的抗电磁干扰能力,因此需要一种能适应多种形态、重量轻且具有优异电磁波吸收特性的柔性吸波材料。在这项研究中,我们通过湿法成型技术,在玻璃涂层非晶磁性纤维(SF)和类达伦巴赫吸波结构的基础上,开发了一种新型柔性吸波材料(FAM)。通过将高性能吸波纤维与纺织结构相结合,FAM 不仅具有电磁波吸波性能,还具有轻质柔性和形状适应性。本文探讨了湿法成型技术中的工艺参数对 FAM 形成的影响,并通过结构优化研究了宽带吸波材料的构造。厚度为 1.7 毫米(SFs 长度为 8 毫米,含量为 3 克/平方米)的单层 FAM 在 11.6 千兆赫频率下达到了令人印象深刻的 -60.1 分贝反射损耗(RL)值。此外,优化的多层 FAM 在 3 至 14 千兆赫的宽范围内实现了有效吸收带宽(EAB:RL ≤ -5 dB)。这项研究提出了一种基于纤维和纺织品结构开发 "轻、薄、宽、强 "吸波材料的新方法,对民用电磁干扰防护和军用电磁隐身技术具有重要意义。
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引用次数: 0
Citrate ions-modified NiFe layered double hydroxide for durable alkaline seawater oxidation 柠檬酸根离子改性的 NiFe 层状双氢氧化物用于持久的碱性海水氧化。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1016/j.jcis.2024.10.086
Seawater electrolysis taking advantage of coastal/offshore areas is acknowledged as a potential way of large-scale producing H2 to substitute traditional technology. However, anodic catalysts with high overpotentials and limited lifespans (caused by chloride-induced competitive chemical reactions) hinder the system of seawater electrolysis for H2 production. Herein, we present a citrate anion (CA) modified NiFe layered double hydroxide nanosheet array on nickel foam (NiFe LDH@NiFe-CA/NF), which serves as an efficient and stable electrocatalyst towards long-term alkaline seawater oxidation. It requires only a low overpotential of 387 mV to achieve a current density of 1000 mA cm−2, outperforming NiFe LDH/NF (414 mV). Moreover, NiFe LDH@NiFe-CA/NF exhibits continuous oxygen evolution testing for 300 h at 1000 mA cm−2 due to its anti-corrosion characterization. Additionally, the fabricated cell can stably operate at 300 mA cm−2 (60 °C, 6 M KOH + seawater) and only require 1.69 V, achieving low energy consumption of seawater splitting.
利用沿海/近海地区的优势进行海水电解,被认为是大规模生产 H2 以替代传统技术的一种潜在方法。然而,阳极催化剂过电位高、寿命有限(由氯离子引起的竞争性化学反应造成),阻碍了海水电解生产 H2 的系统。在此,我们提出了一种柠檬酸阴离子(CA)修饰的泡沫镍上的镍铁层双氢氧化物纳米片阵列(NiFe LDH@NiFe-CA/NF),它是一种高效稳定的电催化剂,可用于长期碱性海水氧化。它只需要 387 mV 的低过电位就能达到 1000 mA cm-2 的电流密度,优于 NiFe LDH/NF(414 mV)。此外,由于具有抗腐蚀特性,NiFe LDH@NiFe-CA/NF 还能在 1000 mA cm-2 电流密度下连续进行 300 小时的氧进化测试。此外,所制造的电池可在 300 mA cm-2 (60 °C、6 M KOH + 海水)条件下稳定运行,且仅需 1.69 V 电压,实现了海水分馏的低能耗。
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引用次数: 0
Assembly and jamming of polar additive-swollen microgels at liquid–liquid interfaces: From inverse Pickering emulsions to functional materials 极性添加剂膨胀微凝胶在液-液界面上的组装和堵塞:从反皮克林乳液到功能材料。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1016/j.jcis.2024.10.051

Hypothesis

Poly-N-isopropylacrylamide (PNIPAM)-based microgels have garnered significant interest as effective soft particulate stabilizers because of their deformability and functionality. However, the inherent hydrophilic nature of microgel restricts their potential use in stabilizing water-in-oil (W/O) Pickering emulsions. Employing diverse polar additives can improve the hydrophobicity of microgels, thus unlocking new possibilities in inverse Pickering emulsion formation and materials fabrication.

Experiments

Different types of microgels were generated using free-radical precipitation polymerization with tailored physiochemical properties. The effect of various polar additives on the wettability, adsorption kinetics, and interfacial coverage of microgels was systematically investigated. Additive-swollen microgels were utilized to stabilize inverse W/O Pickering emulsions, which served as templates to develop functional materials with stimuli responsiveness and hierarchical structures.

Findings

Additive-swollen PNIPAM-based microgels exhibited enhanced hydrophobicity and superior emulsifying capability, which spontaneously assembled and jammed at oil–water interfaces, resulting in a significant interfacial energy decrease. The additive-swollen microgels formed a tightly packed, elastic, and responsive microgel monolayer. The feasibility of the strategy was verified by preparing various inverse W/O Pickering emulsions and high internal phase Pickering emulsions (HIPPEs). More importantly, this straightforward formation strategy of microgel-stabilized inverse W/O Pickering emulsions offered a novel platform to create functional materials with customized inner structures from microscale (e.g., responsive core–shell hydrogel microspheres and colloidosomes) to macroscale (e.g., hierarchical porous materials) that can be used for potential applications, such as recyclable contaminant removal and droplet manipulation.
假设:基于聚-N-异丙基丙烯酰胺(PNIPAM)的微凝胶因其可变形性和功能性而成为有效的软颗粒稳定剂,引起了人们的极大兴趣。然而,微凝胶固有的亲水性限制了其在稳定油包水型(W/O)皮克林乳液中的潜在用途。使用不同的极性添加剂可以改善微凝胶的疏水性,从而为反向皮克林乳液的形成和材料制造提供新的可能性:实验:利用自由基沉淀聚合生成了不同类型的微凝胶,这些微凝胶具有量身定制的理化特性。实验:采用自由基沉淀聚合法生成了不同类型的微凝胶,这些微凝胶具有量身定制的理化特性。系统研究了各种极性添加剂对微凝胶的润湿性、吸附动力学和界面覆盖率的影响。利用添加剂溶胀的微凝胶稳定了反向 W/O 皮克林乳液,并以此为模板开发出了具有刺激响应性和分层结构的功能材料:添加剂溶胀的 PNIPAM 基微凝胶具有更强的疏水性和更优越的乳化能力,能在油水界面自发聚集和堵塞,从而显著降低界面能。添加剂膨胀后的微凝胶形成了一个紧密堆积、富有弹性和反应灵敏的微凝胶单层。通过制备各种反向 W/O 皮克林乳液和高内相皮克林乳液(HIPPE),验证了该策略的可行性。更重要的是,这种直接形成微凝胶稳定的反向 W/O 皮克林乳液的策略提供了一个新颖的平台,可用于创建具有定制内部结构的功能材料,从微观尺度(如响应性核壳水凝胶微球和胶体)到宏观尺度(如分层多孔材料),这些材料可用于可回收的污染物去除和液滴操纵等潜在应用。
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引用次数: 0
Manipulating the d-band center of bimetallic molybdenum vanadate for high performance aqueous zinc-ion battery. 操纵双金属钒酸钼的 d 波段中心,实现高性能水性锌离子电池。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1016/j.jcis.2024.10.073
Youcun Bai, Zhixian Wu, Qidong Lv, Wei Sun, Wenhao Liang, Xin Xia, Heng Zhang, Chang Ming Li

Vanadium-based oxides have good application prospects in aqueous zinc ion batteries (AZIBs) due to their structures suitable for zinc ion extraction and intercalation. However, their poor conductivity limits their further development. The d-band center plays a key role in promoting adsorption of ions, which promotes the development of electrode materials. Here, a series of MoV2O8 compounds with oxygen defect (Od-MoV2O8) were synthesized by a simple hydrothermal process and a subsequent vacuum calcination process through strict control of the deoxidation time. Theoretical calculations reveal that the abundant oxygen vacancies in MoV2O8 effectively regulate the d-band center of the zinc ion adsorption site. This precise control of the d-band center enhances the zinc ion adsorption energy of MoV2O8, lowers the migration energy barrier for zinc ions, and ultimately significantly boosts zinc storage performance. The specific capacity is as high as 282.4 mAh/g after 100 cycles at 0.1 A/g, and it also shows excellent performance and outstanding cycle life. In addition, the maximum energy density of Od-MVO-0.5 (MoV2O8 sample deoxidized for 0.5 h) is 343.3 Wh kg-1. Importantly, the mechanism of Zn2+ storage in Od-MoV2O8 was revealed by the combination of in situ and ex situ characterization techniques.

钒基氧化物具有适合锌离子萃取和插层的结构,因此在锌离子水电池(AZIB)中具有良好的应用前景。然而,它们较差的导电性限制了它们的进一步发展。d 带中心在促进离子吸附方面起着关键作用,从而推动了电极材料的发展。本文通过简单的水热法合成了一系列具有氧缺陷的 MoV2O8 化合物(Od-MoV2O8),并在随后的真空煅烧过程中严格控制脱氧时间。理论计算显示,MoV2O8 中丰富的氧空位可有效调节锌离子吸附位点的 d 带中心。这种对 d 带中心的精确控制增强了 MoV2O8 的锌离子吸附能,降低了锌离子的迁移能垒,最终显著提高了锌的储存性能。在 0.1 A/g 条件下循环 100 次后,比容量高达 282.4 mAh/g,而且性能优异,循环寿命长。此外,Od-MVO-0.5(MoV2O8 样品脱氧 0.5 h)的最大能量密度为 343.3 Wh kg-1。重要的是,通过原位和非原位表征技术的结合,揭示了 Zn2+ 在 Od-MoV2O8 中的储存机制。
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引用次数: 0
Superhydrophobic and super-stretchable conductive composite hydrogels for human motion monitoring in complex condition 用于复杂条件下人体运动监测的超疏水和超拉伸导电复合水凝胶。
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1016/j.jcis.2024.10.069
With the advent of the information age, there is a growing demand for wearable sensing devices. Conventional hydrogels are a class of materials that can hold a large amount of water, with a three-dimensional network of hydrophilic polymerization chains inside. In remote areas or harsh environments, there is an urgent demand for a flexible sensor that is environmentally stable, wearable, and has high mechanical properties. Due to the hydrophilicity of the traditional hydrogel surface, it is easy to adsorb dust or be contaminated by liquid, which limits its further application. As a result, the superhydrophobic hydrogel F-PTD was designed using SiO2@PDA, F-HNT and PT hydrogel. TGA, XPS, SEM, EDS, FT-IR was used to characterize the structure of F-PTD, respectively. Based on the study of mussels, the adhesion property of polydopamine was utilized as an adhesion agent between organic–inorganic interfaces while improving the roughness of the hydrogel surface. The fabricated F-PTD superhydrophobic conductive hydrogels have excellent stretchability (Tensile Strain > 500 %), stable hydrophobicity (CA > 150°), and sensitive electrical conductivity (GF = 3.49). The contact angle of F-PTD is greater than 150° for tensile strains in the range of 0–350 %, and it maintains superhydrophobic under corrosive solutions with pH = 1–14. This enables F-PTD to perform the sensing function of detecting human body signals under complex environmental conditions, which has great potential for application in the field of underwater rescue, wearable electronics and human–computer interfaces.
随着信息时代的到来,人们对可穿戴传感设备的需求日益增长。传统的水凝胶是一类能容纳大量水分的材料,内部有亲水性聚合链组成的三维网络。在偏远地区或恶劣环境中,人们迫切需要一种环境稳定、可穿戴、机械性能高的柔性传感器。由于传统水凝胶表面的亲水性,它很容易吸附灰尘或被液体污染,这限制了它的进一步应用。因此,利用 SiO2@PDA、F-HNT 和 PT 水凝胶设计了超疏水水凝胶 F-PTD。分别采用 TGA、XPS、SEM、EDS 和 FT-IR 对 F-PTD 的结构进行了表征。根据对贻贝的研究,利用聚多巴胺的粘附特性作为有机-无机界面之间的粘附剂,同时改善水凝胶表面的粗糙度。制成的 F-PTD 超疏水导电水凝胶具有优异的拉伸性(拉伸应变 > 500%)、稳定的疏水性(CA > 150°)和灵敏的导电性(GF = 3.49)。F-PTD 的接触角在 0-350 % 的拉伸应变范围内均大于 150°,而且在 pH = 1-14 的腐蚀性溶液中仍能保持超疏水性。这使得 F-PTD 能够在复杂的环境条件下实现探测人体信号的传感功能,在水下救援、可穿戴电子设备和人机界面领域具有巨大的应用潜力。
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引用次数: 0
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Journal of Colloid and Interface Science
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